The bruker high-frequency-EPR system

The design and performance of the first commercial 94 GHz continuous-wave (CW-)/Fourier transform (FT-) EPR and ENDOR spectrometer are described. The spectrometer design is based on a heterodyne microwave bridge using an X-band intermediate frequency (IF), a hybrid magnet system, a variable-temperature, top-loading TeraFlex probehead with a TE₀₁₁ cavity as well as the ELEXSYS-line digital electronics and the Xepr software package. The W-band bridge can be driven by a CW- or pulse-IF unit and delivers a microwave power of 5 mW at 94 GHz. In pulse mode the power is sufficient for a π/2 pulse of 100 ns at a resonatorQ-value of 3000. The magnet system consists of a 6 T split-coil superconducting magnet and a water-cooled room-temperature coil. The main coil can be swept over the full range from 0 to 6 T. The room-temperature coil has a 800 G sweep range around the persistent field of the main magnet. The ENDOR probe features a tuned circuit for¹H nuclei allowing an RF π-pulse of 8 μs with a 200 W amplifier. A broad-band setup is used for other nuclei. The E680 FT-EPR system utilizes the PatternJet pulse programmer and the SpecJet high-speed transient signal averager. The concerted action of these two devices results in a pulse EPR sensitivity equal or higher than in CW-EPR. Selected examples indicating the performance of the 94 GHz CW/FT-EPR and ENDOR systems are shown.     

Experimental study of wave propagation through a rapidly createdplasma

Frequency upconversion and converting a CW source microwave into a frequency upshifted and chirped periodic pulse have been demonstrated by two experiments. In the first one, the CW source microwave propagates through a periodically microwave-discharged plasma. The CW source microwave is converted into a periodic pulse having upshifted carrier frequency. The second one uses a high-voltage (~100-kV) DC discharge to generate a dense plasma suddenly between two parallel plates. A frequency upshifted and chirped pulse (~2 ns) converting from the CW source microwave interacting with the suddenly created plasma is observed. The central frequency (~6.4 GHz) of the pulse is upshifted from the frequency (~4.7 GHz) of the source wave by about 40%. Moreover, frequency components which are upshifted as high as 80% are also observed     

ESR spectrometer with a wide frequency range using a gyrotron as a radiation power source

The development of a high frequency electron spin resonance (ESR) spectrometer with a wide frequency range using a gyrotron as the radiation power source is described.GYROTRON FU-E, optimized for use in an ESR spectrometer in the millimeter wave range, was developed in Fukui University. In order to test the normal operation of the spectrometer, the ESR of two standard samples, single crystal and polycrystalline DPPH, has been measured, in the pulsed mode over the frequency range from 65 GHz to 135 GHz.     

ESR spectrometer with a loop-gap resonator for cw and time resolved studies in a superconducting magnet

The design and performance of an electron spin resonance spectrometer operating at 3 and 9 GHz microwave frequencies combined with a 9-T superconducting magnet are described. The probehead contains a compact two-loop, one gap resonator, and is inside the variable temperature insert of the magnet enabling measurements in the 0-9T magnetic field and 1.5-400 K temperature range. The spectrometer allows studies on systems where resonance occurs at fields far above the g approximately 2 paramagnetic condition such as in antiferromagnets. The low quality factor of the resonator allows time resolved experiments such as, e.g., longitudinally detected ESR. We demonstrate the performance of the spectrometer on the NaNiO2 antiferromagnet, the MgB2 superconductor, and the RbC60 conducting alkaline fulleride polymer.     

A Q-band pulse EPR/ENDOR spectrometer and the implementation of advanced one- and two-dimensional pulse EPR methodology

A versatile high-power pulse Q-band EPR spectrometer operating at 34.5--35.5 GHz and in a temperature range of 4--300 K is described. The spectrometer allows one to perform one- and two-dimensional multifrequency pulse EPR and pulse ENDOR experiments, as well as continuous wave experiments. It is equipped with two microwave sources and four microwave channels to generate pulse sequences with different amplitudes, phases, and carrier frequencies. A microwave pulse power of up to 100 W is available. Two channels form radiofrequency pulses with adjustable phases for ENDOR experiments. The spectrometer performance is demonstrated by single crystal pulse ENDOR experiments on a copper complex. A HYSCORE experiment demonstrates that the advantages of high-field EPR and correlation spectroscopy can be combined and exploited at Q-band. Furthermore, we illustrate how this combination can be used in cases where the HYSCORE experiment is no longer effective at 35 GHz because of the shallow modulation depth. Even in cases where the echo modulation is virtually absent in the HYSCORE experiment at Q-band, matched microwave pulses allow one to get HYSCORE spectra with a signal-to-noise ratio as good as at X-band. Finally, it is shown that the high microwave power, the short pulses, and the broad resonator bandwidth make the spectrometer well suited to Fourier transform EPR experiments.     

HYSCORE and DEER with an upgraded 95GHz pulse EPR spectrometer

The set-up of a new microwave bridge for a 95 GHz pulse EPR spectrometer is described. The virtues of the bridge are its simple and flexible design and its relatively high output power (0.7 W) that generates pi pulses of 25 ns and a microwave field, B(1)=0.71 mT. Such a high B(1) enhances considerably the sensitivity of high field double electron-electron resonance (DEER) measurements for distance determination, as we demonstrate on a nitroxide biradical with an interspin distance of 3.6 nm. Moreover, it allowed us to carry out HYSCORE (hyperfine sublevel-correlation) experiments at 95 GHz, observing nuclear modulation frequencies of 14N and 17O as high as 40 MHz. This opens a new window for the observation of relatively large hyperfine couplings, yet not resolved in the EPR spectrum, that are difficult to observe with HYSCORE carried out at conventional X-band frequencies. The correlations provided by the HYSCORE spectra are most important for signal assignment, and the improved resolution due to the two dimensional character of the experiment provides 14N quadrupolar splittings.     

Analysis of the tuning and operation of reflection resonator EPR spectrometers

This paper investigates basic characteristics of the electron paramagnetic resonance (EPR) signal obtained from spectrometers employing reflection resonators. General equations are presented which reveal the phase and amplitude dependence on instrumental parameters of both components of the continuous wave (CW) EPR signal (absorption and dispersion). New phase vector diagrams derived from these general equations are presented for the analysis of the EPR response. The dependence of the phase and absolute value of the CW EPR signal on the local oscillator (LO) phase and on resonator offset and coupling is presented and analyzed. The EPR spectrometer tuning procedures for both balanced and unbalanced heterodyne receivers are analyzed in detail using the new phase diagrams. Extraneous signals at the RF input of the microwave receiver (resulting from circulator leakage and reflections in the resonator transmission line) have been taken into account and analyzed. It is shown that a final tuning condition that corresponds to an extremum of the receiver output as a function of the resonator frequency is necessary and sufficient for the acquisition of pure absorption signal. This condition is universal: it applies to all spectrometer configurations in all frequency ranges. High Frequency EPR spectrometer (130 GHz) data are used to generate experimental phase diagrams that illustrate the theoretical concepts presented in the paper. Conditions are presented under which the absorption signal can be measured with complete suppression of the dispersion, independent of the mutual frequency offset between the microwave source and the EPR sample resonator. Equations describing the approximate relationship between changes of the resonator properties (Q-factor and frequency) and paramagnetic susceptibility are derived and analyzed.     

Continuous-Wave Operation of a 460-GHz Second Harmonic Gyrotron Oscillator

We report the regulated continuous-wave (CW) operation of a second harmonic gyrotron oscillator at output power levels of over 8 W (12.4 kV and 135 mA beam voltage and current) in the TE(0,6,1) mode near 460 GHz. The gyrotron also operates in the second harmonic TE(2,6,1) mode at 456 GHz and in the TE(2,3,1) fundamental mode at 233 GHz. CW operation was demonstrated for a one-hour period in the TE(0,6,1) mode with better than 1% power stability, where the power was regulated using feedback control. Nonlinear simulations of the gyrotron operation agree with the experimentally measured output power and radio-frequency (RF) efficiency when cavity ohmic losses are included in the analysis. The output radiation pattern was measured using a pyroelectric camera and is highly Gaussian, with an ellipticity of 4%. The 460-GHz gyrotron will serve as a millimeter-wave source for sensitivity-enhanced nuclear magnetic resonance (dynamic nuclear polarization) experiments at a magnetic field of 16.4 T.     

Characterization and suppression of self-phase modulation in a commercial modelocked and Q-switched Nd:YLF oscillator

Spectral broadening up to 20 GHz has been measured in the pulsed output of a commercial actively-modelocked and Q-switched Nd:YLF oscillator operating at a modelocked pulse duration of 150 ps. The source of the broadening is self-phase modulation occurring in the acousto-optic modulators, as confirmed by modeling which has reproduced the observed spectra. With the CW lamp-pumped oscillator redesigned for a large mode volume in the modulators, the self-phase modulation is suppressed and near-transform-limited bandwidths at pulse durations of 85 ps are measured.     

A Dynamic Nuclear Polarization spectrometer at 95 GHz/144 MHz with EPR and NMR excitation and detection capabilities

A spectrometer specifically designed for systematic studies of the spin dynamics underlying Dynamic Nuclear Polarization (DNP) in solids at low temperatures is described. The spectrometer functions as a fully operational NMR spectrometer (144 MHz) and pulse EPR spectrometer (95 GHz) with a microwave (MW) power of up to 300 mW at the sample position, generating a MW B(1) field as high as 800 KHz. The combined NMR/EPR probe comprises of an open-structure horn-reflector configuration that functions as a low Q EPR cavity and an RF coil that can accommodate a 30-50 μl sample tube. The performance of the spectrometer is demonstrated through some basic pulsed EPR experiments, such as echo-detected EPR, saturation recovery and nutation measurements, that enable quantification of the actual intensity of MW irradiation at the position of the sample. In addition, DNP enhanced NMR signals of samples containing TEMPO and trityl are followed as a function of the MW frequency. Buildup curves of the nuclear polarization are recorded as a function of the microwave irradiation time period at different temperatures and for different MW powers.     

外注入非制冷式FP半导体增益开关激光器产生低抖动光脉冲的实验研究

报道了低成本、非制冷法布里-玻罗腔半导体增益开光激光器稳定地产生超短脉冲的实验研究.通过使用外部连续光注入,增益开光激光器的脉冲抖动得到了有效的抑制.实验结果表,明当选择合适功率的连续光注入到非制冷半导体增益开关激光器腔内,可以稳定地产生脉宽26 ps、抖动低于400 fs、重复频率2.5 GHz的脉冲序列.     

Electron paramagnetic resonance W-band spectrometer with a low-noise amplifier

The Mark II W-band (94 GHz) EPR spectrometer with a low-noise millimeter-wave amplifier is described. The microwave bridge is of a high-sensitivity homodyne design. Signal-to-noise ratios were measured for a number of detectors with and without the low-noise amplifier. The signal-to-noise ratio was determined not only by the type of detector but also how well it was matched. Without a microwave preamplifier, a hot-electron bolometer provides the best signal-to-noise ratio. Addition of a low-noise microwave preamplifier to the CW homodyne bridge gives a 10 dB improvement in the noise figure of the receiver at a modulation frequency of 100 kHz. A greater improvement in the signal-to-noise ratio is seen at low modulation frequencies (1–10 kHz), making the low-noise amplifier useful for systems with large linewidths. This allows larger modulation amplitudes to be used without causing significant cavity heating or microphonics. The W-band spectrometer is capable of rapid sweeps from 0 to 7 T, as well as narrower (0.1 T) high-resolution sweeps. It is suitable for a wide variety of samples including liquids and samples cooled to sub-liquid-helium temperatures.     

Generation of 10-GHz ultra-short pulses with low time jitter in an actively mode-locked fiber laser

We have experimentally achieved the 8.3-ps ultra-short pulse at 10 GHz repetition rate with the time jitter as low as 590 fs in an actively mode-locked fiber ring laser. The ring-cavity laser is mode-locked by a semiconductor optical amplifier based on cross-gain modulation. The external CW source is modulated with radio frequency signal by an amplitude modulator as the external optical pulses and, then, injected into the fiber ring cavity to achieve active mode locking. Further investigating the laser output characteristics, it indicates that the linewidth of employed CW source affects properties of the generated ultra-short pulse, such as phase noise and time jitter. Ultra-short pulse at high repetition rate with low time jitter can be generated by the optimization of CW laser source.     

A continuous-wave and pulsed electron spin resonance spectrometer operating at 275 GHz

An electron paramagnetic resonance (EPR) spectrometer is described which allows for continuous-wave and pulsed EPR experiments at 275 GHz (wavelength 1.1 mm). The related magnetic field of 9.9 T for g approximately 2 is supplied by a superconducting solenoid. The microwave bridge employs quasi-optical as well as conventional waveguide components. A cylindrical, single-mode cavity provides a high filling factor and a high sensitivity for EPR detection. Even with the available microwave power of 1 mW incident at the cavity a high microwave magnetic field B1 is obtained of about 0.1 mT which permits pi/2-pulses as short as 100 ns. The performance of the spectrometer is illustrated with the help of spectra taken with several samples.     

Microwave frequency modulation in continuous-wave far-infrared ESR utilizing a quasi-optical reflection bridge

We report the development of the frequency-modulation (FM) method for measuring electron spin resonance (ESR) absorption in the 210- to 420GHz frequency range. We demonstrate that using a high-frequency ESR spectrometer without resonating microwave components enables us to overcome technical difficulties associated with the FM method due to nonlinear microwave-elements, without sacrificing spectrometer performance. FM was achieved by modulating the reference oscillator of a 13GHz Phase-Locked Dielectric Resonator Oscillator, and amplifying and frequency-multiplying the resulting millimeter-wave radiation up to 210, 315 and 420GHz. ESR spectra were obtained in reflection mode by a lock-in detection at the fundamental modulation frequency, and also at the second and third harmonic. Sensitivity of the setup was verified by conduction electron spin resonance measurement in KC60.     

High Power Gyro-Devices for Plasma Heating and Other Applications

Gyrotron oscillators are mainly used as high power millimeter wave sources for electron cyclotron resonance heating (ECRH), electron cyclotron current drive (ECCD), stability control and diagnostics of magnetically confined plasmas for generation of energy by controlled thermonuclear fusion. The maximum pulse length of commercially available 1 MW gyrotrons employing synthetic diamond output windows is 5 s at 110 GHz (CPI and JAERI-TOSHIBA), 12 s at 140 GHz (FZK-CRPP-CEA-TED) and 10 s at 170 GHz (GYCOM and JAERI-TOSHIBA), with efficiencies slightly above 30%. Total efficiencies of 45–50 % have been obtained using single-stage depressed collectors (SDC). The energy world record of 160 MJ (0.89 MW at 180 s pulse length and 140 GHz) at power levels higher than 0.8 MW has been achieved by the European FZK-CRPP-CEA-TED collaboration at FZK. Operation at the 1^st and the 2^nd harmonic of the EC frequency enables gyrotrons to act as medium power step-tunable mm- and sub-mm wave sources in the frequency range from 38 GHz (fundamental) to 889 GHz (2nd harmonic) for plasma diagnostics, EC plasma discharges for generation of multi-charged ions, high-frequency broadband electron paramagnetic resonance (EPR) spectroscopy and medical applications. Gyrotrons have also been successfully used in materials processing. Such technological applications require gyrotrons with the following parameters: f 24 GHz, P_out = 4–50 kW, CW, 30%. Future applications which await the development of novel high-power gyro-amplifiers include high resolution radar ranging and imaging in atmospheric and planetary science as well as deep-space and specialized satellite communications and RF drivers for next-generation high-gradient linear accelerators (supercolliders). The present paper reviews the state-of-the-art and future prospects of gyro-devices and their applications.     

Conduction-electron spin resonance in aluminium by means of a reflection spectrometer at 60 GHz

Conduction-electron spin resonance in thin aluminium platelets, coated with a plastic surface layer, has been studied in a reflection spectrometer at 60 GHz. It is shown that the data on linewidth and g-factor fall in line with recent measurements at 21 GHz by the present authors and partly also with earlier measurements at 1.27 GHz 9.27 GHz, 35 GHz and 79 GHz by others.     

Stochastic excitation and Hadamard correlation spectroscopy with bandwidth extension in RF FT-EPR

The application of correlation spectroscopy employing stochastic excitation and the Hadamard transform to time-domain Fourier transform electron paramagnetic resonance (FT-EPR) spectroscopy in the radiofrequency (RF) band is described. An existing, time-domain FT-EPR spectrometer system with a Larmor frequency (L(f)) of 300 MHz was used to develop this technique by incorporating a pseudo-random pulse sequence generator to output the maximum length binary sequence (MLBS, 10- and 11-bit). Software developed to control the EPR system setup, acquire the signals, and post process the data, is outlined. The software incorporates the Hadamard transform algorithm to perform the required cross-correlation of the acquired signal and the MLBS after stochastic excitation. To accommodate the EPR signals, bandwidth extension was accomplished by sampling at a rate many times faster than the RF pulse repetition rate, and subsequent digital signal processing of the data. The results of these experiments showed that there was a decrease in the total acquisition time, and an improved free induction decay (FID) signal-to-noise (S/N) ratio compared to the conventional coherent averaging approach. These techniques have the potential to reduce the RF pulse power to the levels used in continuous wave (CW) EPR while retaining the advantage of time-domain EPR methods. These methods have the potential to facilitate the progression to in vivo FT-EPR imaging of larger volumes.     

Millimeter wave pulsed gunn oscillator for low chirp radar application at W-Band

Pulsed Gunn oscillator at 94 GHz has been developed using GaAs CW Gunn diode, by choosing a proper operating point and resonant circuit. Peak power output of 25 mw at 94 GHz with a pulse width of 2 microseconds and duty factor of 2% is achieved. Bias circuit oscillations are suppressed by rising the operating voltage alongwith other circuit considerations.     

Evaluation and comparison of pulsed and continuous wave radiofrequency electron paramagnetic resonance techniques for in vivo detection and imaging of free radicals

The performance of two electron paramagnetic resonance (EPR) spectrometers/imagers, one configured in pulsed mode and the other in continuous wave (CW) mode, at an operating frequency of 300 MHz is compared. Using the same resonator (except for altered Q-factors), identical samples and filling factors in the two techniques have been evaluated for their potentials and limitations for in vivo spectroscopic and imaging applications. The assessment is based on metrics such as sensitivity, spatial and temporal resolution, field of view, image artifacts, viable spin probes, and subjects of study. The spectrometer dead time limits the pulsed technique to samples with long phase memories (>275 ns). Nevertheless, for viable narrow-line spin probes, the pulsed technique offers better sensitivity and temporal resolution. The CW technique, on the other hand, does not restrict the choice at spin probes. In addition, the phase-sensitive narrow-band detection of the CW technique gives artifact-free images even for large objects. Selected examples illustrating the performance of the CW and pulsed techniques are presented to put the capabilities of the two techniques in perspective.